Human exposure to particulate matter (PM) has been associated with adverse health effects. While inhalation exposure to airborne PM is a prominent research subject, exposure to PM of geological origin (i.e., generated from soil/soil-like material) has received less attention. This review discusses the contaminants in PM of geological origin and their relevance for human exposure and then evaluates lung bioaccessibility assessment methods and their use. PM of geological origin can contain toxic elements as well as organic contaminants. Observed/predicted PM lung clearance times are long, which may lead to prolonged contact with lung environment. Thus, certain exposure scenarios warrant the use of in vitro bioaccessibility testing to predict lung bioavailability. Limited research is available on lung bioaccessibility test development and test application to PM of geological origin. For in vitro tests, test parameter variation between different studies and concerns about physiological relevance indicate a crucial need for test method standardization and comparison with relevant animal data. Research is recommended on (1) developing robust in vitro lung bioaccessibility methods, (2) assessing bioaccessibility of various contaminants (especially polycyclic aromatic hydrocarbons (PAHs)) in PM of diverse origin (surface soils, mine tailings, etc.), and (3) risk characterization to determine relative importance of exposure to PM of geological origin.